Optical coherence tomography has superior depth penetration, comparable spatial resolution, and superior temporal resolution than any other optical imaging technique, however it lacks the ability to utilize molecular contrast that other optical imaging modalities possess. Molecular contrast provides these techniques with the ability to enhance the contrast of particular tissue morphologies by the administration of contrast agents. It also enables them to record the time evolution of contrast agent concentration, a property extremely useful for drug development and discovery, developmental biology, and clinical diagnostics. We intend to couple proven nonlinear spectroscopic techniques to optical coherence tomography, in order to provide molecular contrast.